For more than 4000 years, paper has been mainly used for the purpose of recording information. With the recent advance in the field of flexible electronics and wearable devices, paper is being investigated as an environmentally friendly alternative to the traditional petrochemical-based polymeric materials. In this work, carbon nanotubes (CNTs) were employed as fillers to produce electrically conductive papers using a typical papermaking process. Lignin was utilized as a renewable dispersant to prepare aqueous suspensions of CNTs and softwood fibers, which served as precursors for sheet fabrication (60 g/m2). CNTs were functionalized to increase the presence of hydroxyl groups and further improve the interfacial strength between CNTs and cellulose fibers through hydrogen bonding. Both tensile strength and breaking length of the papers increased by more than 10% with volume resistivities in the range of 1,600 Ω.cm for CNT loadings as low as 2.5 wt%. The multifunctional sensing behavior of the composite papers to aqueous solutions and tensile strain was thoroughly studied. Results show that the relative electrical resistance significantly increased under water and returned almost to their initial levels after drying, with fast and reproducible signals over multiple immersion/drying cycles. The piezoresistive behavior of the composites increased linearly at low strains followed by an exponential growth at larger strains, and exhibits higher sensitivity than conventional strain gauges. These novel CNT-cellulose composite papers have outstanding multifunctional properties and are promising to be employed for the design of various smart materials, which can revolutionize the way electronic devices are manufactured and used.
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